Novel low-strain layered/rocksalt intergrown cathode for high-energy Li-ion batteries

dc.contributor.authorXu, Len_AU
dc.contributor.authorChen, Sen_AU
dc.contributor.authorSu, Yen_AU
dc.contributor.authorShen, Xen_AU
dc.contributor.authorHe, Jen_AU
dc.contributor.authorAvdeev, Men_AU
dc.contributor.authorKan, WHen_AU
dc.contributor.authorZhang, Ben_AU
dc.contributor.authorFan, Wen_AU
dc.contributor.authorChen, Len_AU
dc.contributor.authorCao, Den_AU
dc.contributor.authorLu, Yen_AU
dc.contributor.authorWang, Len_AU
dc.contributor.authorWang, Men_AU
dc.contributor.authorBao, Len_AU
dc.contributor.authorZhang, Len_AU
dc.contributor.authorLi, Nen_AU
dc.contributor.authorWu, Fen_AU
dc.date.accessioned2025-01-09T22:24:37Zen_AU
dc.date.available2025-01-09T22:24:37Zen_AU
dc.date.issued2023-11-16en_AU
dc.date.statistics2024-07-04en_AU
dc.description.abstractBoth layered- and rocksalt-type Li-rich cathode materials are drawing great attention due to their enormous capacity, while the individual phases have their own drawbacks, such as great volume change for the layered phase and low electronic and ionic conductivities for the rocksalt phase. Previously, we have reported the layered/rocksalt intergrown cathodes with nearly zero-strain operation, while the use of precious elements hinders their industrial applications. Herein, low-cost 3d Mn4+ ions are utilized to partially replace the expensive Ru5+ ions, to develop novel ternary Li-rich cathode material Li1+x[RuMnNi]1-xO2. The as-designed Li1.15Ru0.25Mn0.2Ni0.4O2 is revealed to have a layered/rock salt intergrown structure by neutron diffraction and transmission electron microscopy. The as-designed cathode exhibits ultrahigh lithium-ion reversibility, with 0.86 (231.1 mAh g-1) out of a total Li+ inventory of 1.15 (309.1 mAh g-1). The X-ray absorption spectroscopy and resonant inelastic X-ray scattering spectra further demonstrate that the high Li+ storage of the intergrown cathode is enabled by leveraging cationic and anionic redox activities in charge compensation. Surprisingly, in situ X-ray diffraction shows that the intergrown cathode undergoes extremely low-strain structural evolution during the charge-discharge process. Finally, the Mn content in the intergrown cathodes is found to be tunable, providing new insights into the design of advanced cathode materials for high-energy Li-ion batteries. © 2024 American Chemical Society.en_AU
dc.description.sponsorshipThis work was sponsored by the National Key R&D Program of China (2021YFC2902905), National Natural Science Foundation of China (22109010, U1930102, 11805034), Beijing Nova Program, Chongqing Outstanding Youth Fund (2022NSCQ-JQX3895), Chongqing Talents Plan for Young Talents (CQYC202005032), the Key Project of Chongqing Technology Innovation and Application Development (2022TIAD-DEX0024); N. Li acknowledges the support from Beijing Institute of Technology Research Fund Program for Young Scholars. The authors thank Australian Nuclear Science and Technology Organisation for support with the neutron powder diffraction experiments. The authors greatly appreciate Taiwan Photon Source (TPS) Beamlines 44A1 and 41A1 for the allocation of synchrotron beam time, and local support in data collection and analysis from Prof. Di-Jing Huang, Dr. Chih-Wen Pao, Dr. Hsiao-Yu Huang, Dr. Jun Okamoto, Dr. Amol Singh, and Dr. Jeng-Lung Chen.en_AU
dc.format.mediumPrint-Electronicen_AU
dc.identifier.citationXu, L., Chen, S., Su, Y., Shen, X., He, J., Avdeev, M., Kan, W. H., Zhang, B., Fan, W., Chen, L., Cao, D., Lu, Y., Wang, L., Wang, M., Bao, L., Zhang, L., Li, N., & Wu, F. (2023). Novel low-strain layered/rocksalt intergrown cathode for high-energy Li-ion batteries. ACS Applied Materials & Interfaces, 15(47), 54559-54567. doi:10.1021/acsami.3c13858en_AU
dc.identifier.issn1944-8244en_AU
dc.identifier.issn1944-8252en_AU
dc.identifier.issue47en_AU
dc.identifier.journaltitleACS Applied Materials & Interfacesen_AU
dc.identifier.pagination54559-54567en_AU
dc.identifier.urihttps://doi.org/10.1021/acsami.3c13858en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15880en_AU
dc.identifier.volume15en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Society (ACS)en_AU
dc.subjectCathodesen_AU
dc.subjectLithiumen_AU
dc.subjectLithium ion batteriesen_AU
dc.subjectIonsen_AU
dc.subjectNeutron diffractionen_AU
dc.subjectElectron microscopesen_AU
dc.subjectSpectroscopyen_AU
dc.subjectNickelen_AU
dc.subjectManganeseen_AU
dc.subjectRutheniumen_AU
dc.subjectElectrodesen_AU
dc.subjectRedox reactionsen_AU
dc.titleNovel low-strain layered/rocksalt intergrown cathode for high-energy Li-ion batteriesen_AU
dc.typeJournal Articleen_AU
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